The Super Hero Squad Show premiered in 2009, and originally aired on the Cartoon Network. It was based on the Marvel Super Hero Squad action figure line from Hasbro, which portrays all the characters in the Marvel Universe in a super-deformed-style, and was aimed at a younger generation. The show featured a lot of characters from the Marvel Universe, but primarily focused on a team of heroes including members of the Avengers and the X-Men. It was mostly a parody of super hero shows, and I doubt it ever wanted to be taken too seriously. The story-arc for the first season was about the "Squaddies" trying to stop Doctor Doom's Lethal Legion from collecting the Infinity Fractals, shards from the broken Infinity Sword, which Doom plans on using to rule the world.

Loki here was voiced by Ted Biaselli and first appeared in "Tremble at the Might of MODOK!" In this episode, MODOK is tired of being Doctor Doom's minion and gets his chance to overthrow Doom when an Infinity Fractal gets stuck in his headgear, causing him to grow larger and giving him new abilities like being able to suck the powers from other heroes and villains. Loki approaches him and offers to become his BFF (best fiend forever), but is secretly planning on using MODOK to carry out his own plans regarding the Fractals. Doom tries to take back control and manages to steal Loki's staff and then tricks MODOK into eating some ice cream, which causes him brain-freeze. With MODOK now weakened, the Squaddies manage to remove the Fractal from his head, returning everything to normal. Thor has a short fight with Loki and chases him back to Asgard. There are a couple of neat scenes this episode - for example, Loki turning Thor's winged helmet into a bird, or Loki's reaction to the now giant-MODOK calling him an imp ("My cousin called me an imp once. To this day he doesn't walk right"). Other than that, Loki didn't really get to do anything memorable but overall the episode was good.

"Oh, Brother!" marks Loki's next appearance on the show. This time the God of Mischief convinces Doctor Doom to loan him a couple of his henchmen (like MODOK and Sabretooth), to launch an attack on Asgard alongside his army of Frost Giants, promising Doom some of the warriors of Asgard in return for his help. While most of the Squaddies spend the episode trying to break into Doom's headquarters and take back all the Infinity Fractals he has gathered so far, Thor is called back to his land to fight Loki's army; he is followed by Wolverine, Falcon and Reptil. The short confrontation between Loki and Thor is pretty hilarious - with the former teasing the latter ("You don't even have a real weapon! What are you gonna do, build me a tree-house with your hammer?"), and then making fun of Thor's usual speech pattern ("Bro, seriously. When art thou gonna stop talking like that? Really, we're in the 21st century."). It is later revealed that all this was a diversion Loki came up with to keep everyone busy while he finds a Fractal that was supposedly hidden in the Frost Giant's armory. A Fractal which turns Wolverine into his namesake animal, before Loki takes it for himself. MODOK reports to Doom about Loki's double-cross, but Doom reveals he was expecting this to happen, and transports the other heroes to Loki's hideout. The episode ends with Hulk getting ready to smash the God of Mischief. All in all, a pretty good episode.

Loki is next seen in the episode titled "Support Your Local Sky-Father" where he poses as Gyros the Greek God of Pitas and tricks Zeus into holding a contest between Thor and Hercules after telling him that on Earth, Thor has become more popular than his son. The rivalry between Zeus and Odin forces the two heroes to confront each other in a series of five challenges (most of the based on the mythological Twelve Labors of Hercules, but also an obstacle race). Sue Storm the Invisible Girl is secretly sent to Mount Olympus by the Mayor of Super Hero City to film this competition; broadcasting such an event would have solved the city's financial problems. Sue is the one who discovers Loki is behind everything but as soon as she tries to warn the others the Trickster of Asgard catches her and uses a spell to make her sleep. Meanwhile, Thor and Hercules are tied with two victories each, and the final challenge would settle the winner. Zeus and Odin (wearing special caps with their son's names on them) continue to argue about who will win, until Loki reveals himself and takes control over the two sky-fathers thanks to the caps they were wearing, sending them to battle their sons - once they are all out of his way, he'd rule both Asgard and Olympus! Thor battles Loki while Hercules and the rest of the Squaddies are keeping Zeus and Odin occupied; the battle between the Thunder God and the Trickster God featured in this episode was pretty cool but I thought it was too short. Loki is defeated when the head of a statue of Zeus falls on top of him, knocking him out and breaking the spell cast on Zeus and Odin. In the end everyone reconciles; Thor and Hercules are playing their guitars aboard the SHIELD Helicarrier, while Odin and Zeus agree to go punish Loki together.

In "Lo, How the Mighty Hath Abdicated!" Amora the Enchantress uses a magic love lutefisk to make Odin fall in love with her, thinking this would make her the queen of Asgard. For a change this wasn't a scheme orchestrated by Loki, but he does find a way to take advantage of the situation: according to the rules, by marrying a commoner Odin has in fact abdicated and is no longer the king of Asgard. Next in line for the throne should be Thor, Odin's first born son but since he is busy helping the Super Hero Squad in their fight with Thanos (who became the main villain in the first half of the second season), Loki claims that he should be crowned king. However Thor learns about the Enchantress becoming his new mother and arrives in Asgard just in time to claim the throne. There are a couple of funny scenes, like Hogun the Grim meeting the Squaddies (and mentioning how they have always been "Hogun's heroes"), or Thor saying goodbye to his friends so that he can stay in Asgard (telling Iron Man "I'm going to miss you the most, Tin Man"). Loki tries destroying Thor a couple of times so he can take his place as king, but all his plans backfire with comedic results. Amora comes up with a new scheme: Odin might not be king anymore but he's still the most powerful Assgardian, so he sends him to destroy king Thor and prince Loki - and claim the throne afterwards. However, Odin's love for Thor apparently breaks Amora's spell and he returns to normal (though Loki wasn't so lucky; he was blasted through a wall a couple of times thanks to the Odinforce). Odin divorces Amora and regains his status as king of Asgard. The episode also features a sub-plot about Magneto and Quicksilver attacking the Helicarrier trying to rescue Wanda the Scarlet Witch, thinking she's a prisoner there (she actually became one of the good guys and joined the Squad earlier during the season). Overall, a pretty great episode.